We report a significant enhancement of the Schottky barrier height of Au/N–ZnS0.07Se0.93 diodes formed by the cryogenic process. The improvement is around 25%. This technique had previously been successfully applied to some narrow band gap semiconductors, such as InP and InGaAs. We explain this improvement by the metal–insulator–semiconductor model and the uniformity of the metal film so‐obtained. This technique is proven to be of importance for making low dark/leakage current visible light sensitive optoelectronic devices.

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